Process for the manufacturing of dense silicon carbide

a technology of dense silicon carbide and manufacturing process, which is applied in the field of producing dense silicon carbide articles, can solve the problems of cost-prohibition, difficult operation and control, and cost-prohibition of conventional ceramic processes, and achieve the effects of reducing open porosity and improving most chemical, mechanical and thermal properties

Inactive Publication Date: 2006-01-05
POCO GRAPHITE
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0011] As an embodiment of the present invention, a method of producing a densified SiC (silicon carbide) article is advantageously provided. In this embodiment, a porous SiC preform is provided. A preform is an article that can be formed to finish form. In all embodiments of the present invention, the porous SiC preform can be formed starting with a graphite block that has an open porosity. The graphite block can be machined into a near-net shape graphite article. The term near-net shape is used here to indicate that the part will require only minimal post machining to meet final tolerances. The term preform encompasses near-net shape articles. The graphite preform can then be contacted with silicon monoxide gas at a first preselected temperature to form the porous silicon carbide preform. A substantial number of pores within the porous silicon carbide preform are then filled with a carbon precursor to produce a filled silicon carbide preform. The filled silicon carbide preform is then heated at a second preselected temperature to polymerize the carbon precursor contained within the filled silicon carbide preform to form a polymerized filled silicon carbide preform. The polymerized filled silicon carbide preform is further heated at a third preselected temperature to produce a carbonaceous porous structure within the pores of the porous silicon carbide preform. The carbonaceous porous structure, inside the SiC preform, is then contacted with silicon in an inert atmosphere at a fourth preselected temperature and a first preselected pressure. In this step, the silicon wicks through the carbonaceous porous structure and reacts with carbon contained within the pores of the porous silicon carbide preform to produce silicon carbide within the pores of the porous silicon carbide preform. The produced densified silicon carbide is characterized by having no or substantially reduced open porosity. The elimination or substantial reduction in porosity will significantly improve most chemical, mechanical and thermal properties including but not limited to oxidation resistance, strength, stiffness, thermal conductivity, and thermal stability of SiC articles produced using the process described in this invention.

Problems solved by technology

Conventional processes for the fabrication of near-net shape dense SiC components such as pressureless sintering and hot pressing, and the like are difficult to operate and control and are cost-prohibitive.
Conventional ceramic processes, such as pressureless sintering, for the manufacturing of near-net shape SiC articles are becoming costly due to the increased complexity of some of these SiC components.
Furthermore, the mold has a limited lifetime due to erosion resulting from each use that would cause dimensional changes of the mold, which in turn result in unpredictable dimensions of the sintered SiC product.
The use of coarse SiC particulates presents many problems such as poor thermal shock resistance of the material and poor isotropy.
Prior art processes for manufacturing dense SiC articles are difficult to operate and are expensive.
However, SiC articles produced by the CVR process contain some porosity that could be detrimental to the chemical, mechanical and thermal properties of the SiC product.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

example 1

[0025] A block of porous graphite was produced by Poco Graphite having an average porosity of about 30%. The porous graphite block was machined into 0.25″×2″×2″ tiles and 0.25″×0.5″×4″ bars. The porous graphite tiles and bars were then heated at 1800° C. in the presence of silicon monoxide gas to convert the porous graphite tiles and bars to porous silicon carbide tiles and bars. The porous silicon carbide tiles and bars were then impregnated with a liquid mixture of allylhydridopolycarbosilane (AHPCS) and phenolic resin which upon pyrolysis would produce a solid mixture of silicon carbide and carbon. The impregnated silicon carbide tiles and bars were then heated to a pre-selected second temperature of 150° C. in air to polymerize the silicon carbide / carbon precursor. The tiles and bars were then heated further in an inert atmosphere to 1600° C. to char the polymer and to produce a mixture of silicon carbide and carbon structure inside the pores of the silicon carbide tiles and bar...

example 2

[0026] A block of porous graphite was produced by Poco Graphite having an average porosity of about 30%. The porous graphite block was machined into 0.25″×2″×2″ and 0.25″×4″×4″ porous graphite tiles. The graphite tiles were then heated at 1800° C. in the presence of silicon monoxide gas to convert the graphite tiles to silicon carbide tiles. The porous silicon carbide tiles were then impregnated with a liquid mixture of catalyzed furfuryl alcohol as the carbon precursor and a mixture of diethylene glycol and triethylene glycol as the pore-forming agent. The impregnated silicon carbide tiles were then heated to 90° C. in air to polymerize the furfuryl alcohol. The samples were then further heated in an inert atmosphere to 1000° C. to evaporate the pore-forming agent and char the polymer to produce a carbon structure with interconnected porosity inside the pores of the silicon carbide tiles. This carbonization cycle was repeated one more time to produce more carbon inside the pores of...

example 3

[0027] A block of porous graphite was produced by Poco Graphite having an average porosity of about 30%. The porous graphite block was machined into 0.25″×2″×2″ tiles and 0.25″×0.5″×4″ bars. The graphite tiles and bars were then heated at 1800° C. in the presence of silicon monoxide gas to convert the graphite tiles and bars to silicon carbide tiles and bars. The porous silicon carbide tiles and bars were then heated to about 1000° C. in the presence of methane (CH4) gas as the carbon precursor. The methane gas diffused into the pores and decomposed into solid pyrolytic carbon / graphite and hydrogen gas. The solid carbon / graphite deposited inside the pores of the silicon carbide tiles and bars while the hydrogen gas diffused out of the porous silicon carbide tiles and bars. This process was allowed to continue until the samples gained about 4-5% weight. The carbonized tiles and bars were then infiltrated with liquid silicon at 1650° C. in inert atmosphere to convert the pyrolytic car...

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Abstract

A method of producing a densified SiC article is provided. Near-net shape porous silicon carbide articles are produced and densified using the developed method. A substantial number of pores within the porous near-net shape silicon carbide article are filled (impregnated) with a carbon precursor, a silicon carbide precursor, or a mixture of both. The carbon precursor can be liquid or gas. The filled SiC preform is heated to convert the carbon or silicon carbide precursor to porous carbon or SiC preform inside the pores of the net-shape silicon carbide article. The impregnation / pyrolysis cycle is repeated until the desired amount of carbon and / or silicon carbide is achieved. In case of a carbon or a mixture of silicon carbide / carbon precursor is used, the pyrolyzed near-net shape silicon carbide article is then contacted with silicon in an inert atmosphere. The silicon diffuses through the pyrolyzed near-net shape silicon carbide article and reacts with the carbon contained within the pores of the porous SiC preform producing a new phase of silicon carbide within the pores of the near-net shape silicon carbide article. The produced silicon carbide is a near-net dense silicon carbide article.

Description

RELATED APPLICATIONS [0001] This patent application claims priority to U.S. Provisional Patent Application Ser. No. 60 / 584,244 filed on Jun. 30, 2004, which is incorporated by reference in its entirety.BACKGROUND OF THE INVENTION [0002] 1. Technical Field of the Invention [0003] The present invention relates to a method of producing silicon carbide articles. [0004] 2. Description of the Related Art [0005] Silicon carbide (SiC) or moissanite is a ceramic compound consisting of carbon and silicon. SiC was accidentally discovered by Edward G. Acheson, an assistant to Thomas Edison, about 1890, when he was running an experiment on the synthesis of diamonds. Acheson thought the new material was a compound of carbon and alumina, present in the clay, leading him to name it carborundum, a name that is still being used on some occasions. SiC occurs naturally in meteorites, though very rarely and in very small amounts. Being the discoverer of SiC, Acheson was the first to synthesize SiC by pa...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): B05D3/02
CPCC04B35/573C04B38/0022C04B2235/9607C04B2235/96C04B2235/95C04B2235/77C04B2235/72C04B2235/616C04B38/0032C04B2111/00905C04B2111/2084C04B2235/48C04B2235/483C04B2235/614C04B35/565C04B41/5059C04B35/52C04B38/0058
Inventor RASHED, ABUAGELA H.SHEPPARD, REX G.BRAY, DONALD J.
Owner POCO GRAPHITE
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